US8951688B2 - Method and device for increasing the service life of a proton exchange membrane fuel cell - Google Patents

Method and device for increasing the service life of a proton exchange membrane fuel cell Download PDF

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Publication number
US8951688B2
US8951688B2 US13/379,674 US201013379674A US8951688B2 US 8951688 B2 US8951688 B2 US 8951688B2 US 201013379674 A US201013379674 A US 201013379674A US 8951688 B2 US8951688 B2 US 8951688B2
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cell
fuel cell
performance
electrodes
reversal
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Expired - Fee Related, expires
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US20120183874A1 (en
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Alejandro Franco
Olivier Lemaire
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Commissariat a lEnergie Atomique et aux Energies Alternatives CEA
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Commissariat a lEnergie Atomique et aux Energies Alternatives CEA
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/043—Processes for controlling fuel cells or fuel cell systems applied during specific periods
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04223—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids during start-up or shut-down; Depolarisation or activation, e.g. purging; Means for short-circuiting defective fuel cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M2008/1095—Fuel cells with polymeric electrolytes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • the present invention is situated in the field of proton exchange membrane fuel cells, well known under the acronym PEMFC.
  • the present invention is based on a reversal of the functioning of the cell.
  • PEMFCs are current generators the operating principle of which, illustrated in FIG. 1 , is based on the conversion of chemical energy into electrical energy, by catalytic reaction of hydrogen and oxygen.
  • Membrane-electrode assemblies or MESs 1 constitute the basic elements of PEMFCs. They are composed of a polymer membrane 2 and catalytic layers 3 , 4 present on either side of the membrane 2 and constituting respectively the anode and cathode.
  • the membrane 2 therefore separates the anodic 5 and cathodic 6 compartments.
  • the catalytic layers 3 , 4 generally consist of platinum nanoparticles supported by carbon aggregates.
  • Gaseous diffusion layers 7 , 8 (carbon fabric, felt, etc.) are arranged on either side of the MES 1 in order to provide the electrical conduction, the homogeneous distribution of the reactive gases and the discharge of the water produced by the reaction.
  • a system of channels 9 , 10 placed on either side of the MES brings in the reactive gases and discharges the water and excess gases to the outside.
  • the decomposition of the hydrogen adsorbed on the catalyst produces protons H + and electrons e 31 .
  • the protons then pass through the polymer membrane 2 before reacting with the oxygen at the cathode 4 .
  • the reaction of the protons with the oxygen at the cathode leads to the formation of water and the production of heat ( FIG. 2 ).
  • the potential of this reaction (1) is approximately 0.2 V/SHE. Given that the cathodic potential of a cell is generally greater than 0.2 V, this reaction always takes place.
  • the oxygen present at the anode 3 is normally reduced by the hydrogen in the anodic compartment.
  • the hydrogen is not sufficient to reach the oxygen.
  • the oxygen still present has recourse to other sources of protons and, in particular, to those produced by the oxidation of the cathodic carbon.
  • the oxygen present at the anode 3 therefore acts as a proton (“proton pump effect”) that accentuates the corrosion of the carbon at the cathodic catalytic layer 4 , and reaction (1) is then strongly moved to the right ( FIG. 3 ): C ⁇ 2H 2 O CO 2 +4H ⁇ +4e ⁇ (2)
  • the degradation of the platinum at the cathode also participates in the reduction of the performance of the cell.
  • One of the degradation mechanisms concerns the oxidation, dissolution and recrystallisation of the platinum.
  • Electrochemical maturation is another platinum degradation mechanism that leads to an increase in the size of the platinum particles.
  • document FR 2 925 229 describes a solution based on a periodic reduction of the temperatures of the cell and humidifiers for a few hours, so as to maintain a stable relative humidity. This solution effectively significantly increases the service life of the cells but requires a temperature control device.
  • the present invention forms part of the search for novel technical solutions for limiting the corrosion of the carbon at the cathode at PEMFCs, and thus prolonging the service life thereof.
  • the present invention proposes to reverse the functioning of the cell. Since the deterioration of the electrodes is not symmetrical, reversal firstly protects the deteriorated cathode, which then functions correctly as an anode, and secondly makes it possible to use the non-affected anode as a new cathode. It is clear that the present invention constitutes an inexpensive technical solution that is simple to implement.
  • the present invention concerns a method of using a fuel cell of the PEMFC type consisting in performing at least one reversal of the functioning of the cell during use thereof.
  • the cell being composed of a polymer membrane and electrodes, namely an anode and a cathode, it is recommended exchanging the respective roles of these electrodes.
  • the electrode that fulfilled the role of anode becomes the cathode and conversely the electrode that fulfilled the roll of cathode becomes the anode.
  • the invention concerns a method of using a fuel cell of the PEMFC type, composed of a polymer membrane and electrodes present on either side of the membrane, which comprises the following steps:
  • performance means advantageously the potential (U) of the cell.
  • This reversal operation can be repeated until the cell collapses, that is to say the potential collapses.
  • the functioning of the cell is reversed by means of a physical reversal of the cell. It is therefore a case of physically exchanging the electrodes, that is to say an at least partial movement of the device. In practice, it is a case of dismantling the cell and turning over the cell core (the MES assembly) and then reclosing the cell.
  • the service life of the cell can be at least doubled.
  • the reversal is repeated, that is to say it is performed at least twice during the use of the cell.
  • the moment chosen for the reversal can be determined in different ways:
  • This embodiment requires monitoring of the potential of the cell over time.
  • the cell is therefore connected to a system for measuring the potential.
  • Measurement of the potential in real time can be carried out continuously or at predetermined intervals of time, regular or not. In the case of functioning under pure gases, this measurement can be carried every ten minutes, or even every hour.
  • an impure gas fuel or oxidant
  • it is preferable to increase the frequency of the measurements since the presence of impurities may give rise to a rapid plunge in the performance.
  • the measurement of the potential is then advantageously carried out at a minimum every minute.
  • At least one reversal is performed.
  • the reversal be repeated on several occasions and therefore repetitive, optionally randomly or by applying one or other or both of the criteria stated above (according to the potential or time).
  • the threshold values applied may remain constant throughout the use or may vary.
  • the reversal of the gas supply to the electrodes can be carried out by means of the arrangement of the cell on a rotary platform. It is then necessary to disconnect the cell from its supply system, for example by means of quick couplings. The platform then drives the cell in a half turn so that the cathode is in the anode position and the anode is in the cathode position.
  • each electrode is provided with a dual gas supply system and advantageously a means of controlling the supply.
  • each can be supplied with fuel, in particular hydrogen, and oxidant, in particular oxygen and/or air, respectively.
  • the nature of the gas supplying the electrode determines the function thereof.
  • the gas supply system is advantageously cleaned, preferably by circulation of a neutral gas, before each reversal.
  • the control system makes it possible to activate one or other of the gas supply systems. It advantageously consists of valves. At the time of reversal of functioning, the position of the valves is changed, which results in a reversal of the gas supply to each electrode.
  • a dual discharge system is also provided with a control system for selecting the routing of the discharge of the gases.
  • a control system for selecting the routing of the discharge of the gases.
  • the system for controlling the supply and discharge of gases for the electrodes is connected to a system for measuring the potential of the cell or the operating time of the cell. Under these conditions, the interchange takes place automatically.
  • FIG. 1 shows the diagram of the principle of a fuel cell of the PEMFC type.
  • FIG. 2 shows the initial functioning of a fuel cell of the PEMFC type.
  • FIG. 3 shows the functioning of a fuel cell of the PEMFC type after several hundred hours.
  • FIG. 4 shows the functioning of a fuel cell of the PEMFC type after reversal of the electrodes.
  • FIG. 5 shows schematically a device according to the invention provided with valves according to a first configuration (A) or a second configuration (B).
  • FIG. 6 illustrates the change in potential of the cell as a function of time, in the case of reversal performed when the performance of the cell goes below a predetermined threshold.
  • FIG. 7 illustrates the change in the potential of the cell as a function of time, in the case of a reversal performed when the performance of the cell has fallen.
  • FIG. 8 illustrates the change in the potential of the cell as a function of time, in the case of a reversal repeated over time.
  • FIG. 9 shows schematically a device according to the invention provided with a rotary platform according to a first configuration (A) or a second configuration (B).
  • the initial operating diagram of a fuel cell 1 is illustrated in FIG. 2 .
  • the cathodic active layer 4 is not degraded.
  • the carbon particles are intact and the catalyst particles are evenly distributed ( FIG. 2 ).
  • the result is good contact resistance and a large active surface.
  • the damage to the carbon carrier at the cathode 4 and the increase in the size of the particles after functioning cause the loss of catalytic surface and an increase in the contact resistance between the cathode 4 and the gaseous diffusion layer 8 . All these phenomena participate in the reduction in the durability of the PEMFCs.
  • the electrode that functioned as the anode 3 becomes the cathode 4 and the electrode that functioned as the cathode 4 becomes the anode 3 .
  • the active layer of the highly-degraded cathode is then replaced by the active layer of the initial anode that is almost intact.
  • each electrode is connected to a dual gas supply system 11 , both at the inlet and the outlet, equipped with valves 12 .
  • the valve system 12 introduces hydrogen into the electrode 1 (then assimilatable to the anode 3 ) and air or oxygen into the electrode 2 (then assimilatable to the cathode 4 ).
  • the valve system at the outlet from the cell sends hydrogen into the system provided for collecting the fuel gases 9 and sends air or oxygen into the system provided for collecting the oxidising gases 10 .
  • valves open in configuration A are closed and the valves closed are open.
  • the hydrogen is then supplied to the electrode 2 (then assimilatable to the anode 3 ) and the air or oxygen is supplied to the electrode 1 (then assimilatable to the cathode 4 ).
  • the valves at the outlet of the cell are also interchanged so that the hydrogen issuing from the electrode 2 can be connected in the system provided for the fuel gas 9 .
  • the air or oxygen issuing from the cell is directed into the system provided for the oxidising gases 10 .
  • the cell is reversed when the performance of the cell has decreased for example by 20% ( FIG. 6 ). There is thus a change from functioning according to configuration A to functioning according to configuration B. The speed of the degradation of the cell potential is decreased.
  • the durability of the fuel cell is increased by at least double compared with the case where the configuration reversal is not applied.
  • the change from configuration A to configuration B is effected at the time of collapse of cell potential resulting from the degradation of its cathode ( FIG. 9 ).
  • the cell potential is increased and the speed of its degradation decreases.
  • the change from configuration A to configuration B is effected repetitively.
  • the speed of the degradation of the cell potential is decreased more and more ( FIG. 8 ).
  • the cell is reversed periodically.
  • the reversal is related neither to a performance threshold (see 2-1-1) nor to an abrupt plunge in the potentials (see 2-1-2).
  • the durability of the fuel cell is increased by at least double compared with the case where the series of configuration reversals is not applied.
  • the cell is supported on a rotary platform 13 for reversing access of the gases.
  • the gas circuit 11 remains in place. It is the cell that moves, being secured to a platform example.
  • the platform 13 then drives the cell in a half turn (180° so that the former cathode (electrode 2 ) is in the anode position and the former anode (electrode 1 ) is in the cathode position.

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  • Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Fuel Cell (AREA)
US13/379,674 2009-07-09 2010-07-09 Method and device for increasing the service life of a proton exchange membrane fuel cell Expired - Fee Related US8951688B2 (en)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
FR0954767A FR2947957B1 (fr) 2009-07-09 2009-07-09 Methode et dispositif pour augmenter la duree de vie d'une pile a combustible a membrane echangeuse de protons
FR0954767 2009-07-09
PCT/FR2010/051458 WO2011004134A1 (fr) 2009-07-09 2010-07-09 Méthode et dispositif pour augmenter la durée de vie d'une pile à combustible à membrane échangeuse de protons

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US20120183874A1 US20120183874A1 (en) 2012-07-19
US8951688B2 true US8951688B2 (en) 2015-02-10

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US (1) US8951688B2 (fr)
EP (1) EP2452388B1 (fr)
JP (1) JP5718328B2 (fr)
ES (1) ES2413680T3 (fr)
FR (1) FR2947957B1 (fr)
WO (1) WO2011004134A1 (fr)

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FR3080458B1 (fr) 2018-04-24 2023-06-23 Commissariat Energie Atomique Procede de detection d’une anomalie de fonctionnement d’une batterie et systeme mettant en oeuvre ledit procede
CN116840722B (zh) * 2023-06-09 2024-02-23 淮阴工学院 一种质子交换膜燃料电池性能退化评估及寿命预测方法

Citations (9)

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EP0692835A2 (fr) 1994-07-13 1996-01-17 Toyota Jidosha Kabushiki Kaisha Générateur à piles à combustible et procédé d'opération
US6030718A (en) * 1997-11-20 2000-02-29 Avista Corporation Proton exchange membrane fuel cell power system
US6068943A (en) * 1996-12-17 2000-05-30 Forschungszeutrum Julich GmbH Fuel cell apparatus and method of increasing the power density of fuel cells using carbon-containing fuels
US20040126629A1 (en) 2002-12-27 2004-07-01 Reiser Carl A. Reversible fuel cell power plant
EP1460704A1 (fr) 2003-03-21 2004-09-22 Bose Corporation Méthode de restauration de la performance d'une pile à combustible par l'utilisation de impulsions de courant inverse et système de pile à combustible correspondant
JP2006278190A (ja) 2005-03-30 2006-10-12 Toyota Central Res & Dev Lab Inc 燃料電池システム
JP2007053012A (ja) 2005-08-18 2007-03-01 Nissan Motor Co Ltd 燃料電池の始動制御装置
US20090155643A1 (en) 2007-12-18 2009-06-18 Commissariat A L'energie Atomique Method for using a fuel cell comprising a regeneration step by lowering the temperature
JP2009181810A (ja) 2008-01-30 2009-08-13 Toyota Motor Corp 燃料電池の運転方法

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JP4016536B2 (ja) * 1999-07-09 2007-12-05 日産自動車株式会社 燃料電池車の出力診断装置
JP3475869B2 (ja) * 1999-09-17 2003-12-10 松下電器産業株式会社 高分子電解質型燃料電池とその特性回復方法
JP4618985B2 (ja) * 2003-05-12 2011-01-26 積水化学工業株式会社 燃料電池システム
WO2005006477A1 (fr) * 2003-07-15 2005-01-20 Aisin Seiki Kabushiki Kaisha Procede de fonctionnement d'une pile a combustible
JP2005235698A (ja) * 2004-02-23 2005-09-02 Toyota Motor Corp 燃料電池
JP3118633U (ja) * 2005-11-16 2006-02-02 岩谷産業株式会社 移動式燃料電池装置

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0692835A2 (fr) 1994-07-13 1996-01-17 Toyota Jidosha Kabushiki Kaisha Générateur à piles à combustible et procédé d'opération
US6068943A (en) * 1996-12-17 2000-05-30 Forschungszeutrum Julich GmbH Fuel cell apparatus and method of increasing the power density of fuel cells using carbon-containing fuels
US6030718A (en) * 1997-11-20 2000-02-29 Avista Corporation Proton exchange membrane fuel cell power system
US20040126629A1 (en) 2002-12-27 2004-07-01 Reiser Carl A. Reversible fuel cell power plant
EP1460704A1 (fr) 2003-03-21 2004-09-22 Bose Corporation Méthode de restauration de la performance d'une pile à combustible par l'utilisation de impulsions de courant inverse et système de pile à combustible correspondant
JP2006278190A (ja) 2005-03-30 2006-10-12 Toyota Central Res & Dev Lab Inc 燃料電池システム
JP2007053012A (ja) 2005-08-18 2007-03-01 Nissan Motor Co Ltd 燃料電池の始動制御装置
US20090155643A1 (en) 2007-12-18 2009-06-18 Commissariat A L'energie Atomique Method for using a fuel cell comprising a regeneration step by lowering the temperature
FR2925229A1 (fr) 2007-12-18 2009-06-19 Commissariat Energie Atomique Procede d'utilisation d'une pile a combustible comportant une etape de regeneration par abaissement de la temperature
JP2009181810A (ja) 2008-01-30 2009-08-13 Toyota Motor Corp 燃料電池の運転方法

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Franco et al., "Multiscale Model of Carbon Corrosion in a PEFC: Coupling with Electrocatalysis and Impact on Performance Degradation," Journal of the Electrochemical Society, 155(4) B367-B384 (2008).
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Also Published As

Publication number Publication date
FR2947957A1 (fr) 2011-01-14
US20120183874A1 (en) 2012-07-19
JP2012533147A (ja) 2012-12-20
EP2452388A1 (fr) 2012-05-16
WO2011004134A1 (fr) 2011-01-13
FR2947957B1 (fr) 2011-08-12
JP5718328B2 (ja) 2015-05-13
ES2413680T3 (es) 2013-07-17
EP2452388B1 (fr) 2013-06-05

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